Perpendicularly magnetized ferromagnetic thin films have applications in permanent magnets, hard disk drive (HDD) devices, nonvolatile memory technologies (e.g., STT-MRAM), sensors, and spintronic devices (e.g., magnetic logic), among others. Various materials, including manganese aluminum (MnAl), have been investigated over the years to determine whether they are suitable for producing thin films having magnetic properties, such as high perpendicular magnetic anisotropy (PMA), suitable for commercial applications. These investigations have revealed that thin MnAl films having L10-ordering (a/k/a the “τ-phase”) appear promising for commercial applications. However, the τ-phase MnAl films achieved to date are not optimal for computing applications, such as HDDs, nonvolatile memory technologies, and spintronic devices, among others. In addition, while there has been considerable work developing τ-MnAl films on substrates such as GaAs (001), MgO (001), and glass since the material was discovered around 1960, there have been no reports of high-PMA τ-MnAl films on Si substrates in spite of the fact that there have been attempts to make them on Si substrates.